Molecular Design for Optically Induced Magnetization: Targeting Excited State Orbital Degeneracy in Tungsten(V) Complexes
Journal of the American Chemical Society,
Год журнала:
2025,
Номер
unknown
Опубликована: Май 20, 2025
The
rise
of
quantum
information
science
has
spurred
chemists
to
prepare
new
molecules
that
serve
as
useful
building
blocks
in
technologies
the
future.
Implementation
molecular
spin-based
qubits
requires
methods
induce
high
spin
polarization
samples.
Herein,
we
report
design
criteria
develop
axially
symmetric
spin-1/2
amenable
optically
induced
magnetization
(OIM),
a
technique
using
circularly
polarized
(CP)
excitation
deliver
polarization.
We
apply
these
series
tungsten(V)
chalcogenide
complexes
are
demonstrated
have
large
spin-sensitive
responses
CP
light
magnetic
circular
dichroism
(MCD)
could
allow
up
∼20%
through
OIM.
Pulsed
electron
paramagnetic
resonance
(EPR)
spectra
reveal
systems
improved
relaxation
times
over
like
K2IrCl6,
species
recently
investigated
by
OIM,
and
field-swept
spin-echo
(FS-ESE)
experiments
show
they
remarkable
lack
anisotropy
their
phase-memory
Tm
times.
general
point
toward
future
ways
improve
OIM-initializable
qubits.
Язык: Английский
Ultrafast all-optical coherence of molecular electron spins in room-temperature water solution
Science,
Год журнала:
2024,
Номер
386(6724), С. 888 - 892
Опубликована: Ноя. 7, 2024
The
tunability
and
spatial
precision
of
paramagnetic
molecules
makes
them
attractive
for
quantum
sensing.
However,
usual
microwave-based
detection
methods
have
poor
temporal
resolution,
optical
compatible
with
room-temperature
solutions
remained
elusive.
In
this
study,
we
utilized
pump-probe
polarization
spectroscopy
to
initialize
track
electron
spin
coherence
in
a
molecule.
Designed
efficiently
couple
spins
light,
aqueous
potassium
hexachloroiridate(IV)
enabled
few-picosecond
free-induction
decay
at
room
temperature
micromolar
concentrations.
Viscosity
was
found
strongly
vary
decoherence
lifetimes.
This
approach
has
improved
the
experimental
time
resolution
by
up
five
orders
magnitude,
making
it
possible
observe
molecular
system
that
only
exhibits
below
25
kelvin
traditional
techniques.
Язык: Английский